Dynamic Cross-Linking of Polymeric Binders Based on Host–Guest Interactions for Silicon Anodes in Lithium Ion Batteries

We report supramolecular cross-linking of polymer binders via dynamic host–guest interactions between hyperbranched β-cyclodextrin polymer and a dendritic gallic acid cross-linker incorporating six adamantane units for high-capacity silicon anodes. Calorimetric analysis in the solution phase indicates that the given host–guest complexation is a highly spontaneous and enthalpically driven process. These findings are further verified by carrying out gelation experiments in both aqueous and organic media. The dynamic cross-linking process enables intimate silicon–binder interaction, structural stability of electrode film, and controlled electrode–electrolyte interface, yielding enhanced cycling performance. Control experiments using both α, γ-CDp with different cavity sizes and a guest molecule incorporating a single adamantane unit verified that the enhanced cycle life originates from the host–guest interaction between β-cyclodextrin and adamantane. The impact of the dynamic cross-linking is maximized at an optimal stoichiometry between the two components. Importantly, the present investigation proves that the molecular-level tuning of the host–guest interactions can be translated directly to the cycling performance of silicon anodes.